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Polydimethylsiloxane & poly(4-methyl-1-pentene) as gutter layer and P84 polyimide coated composite hollow fiber membranes for N₂/CO₂ and CO₂/CH₄ separation

Abstract : Composite membrane structures are inevitable for the next step of mixed matrix membrane development as the commonly used asymmetric membrane design would mean majority of the fillers to be wasted in the bulk porous substrate layer. In this research, the possibility of using poly(4-methyl-1-pentene) (PMP) as substrate – gutter layer in composite membrane was compared with commonly used polydimethylsiloxane (PDMS) as gutter layer, supported on lithium chloride (LiCl) modified polyethersulfone (PES) porous substrate of varying surface pore architectures. Composite PES/PDMS was able to obtain permeance as high as 26.6 ± 2.6 GPU for N2 and 354.4 ± 27.9 GPU for CO2 at about 1 µm minimum coating thickness. Nevertheless, this value is lower than asymmetric dense skin PMP membrane at 84.6 ± 6.2 GPU for N2 and 607.3 ± 31.3 GPU for CO2. Despite that PDMS has intrinsic permeability far higher than PMP, PES/PDMS composite suffers from solution intrusion & geometric restriction problem at its dense – substrate interface, which reduces its permeance efficiency as low as only 4% of its supposedly ideal permeance, at low coating thickness. It is further elucidated that substrate surface uniformity also significantly affects the resulting composite permeance. In comparison, asymmetric PMP with thin dense surface layer was noted to be advantageous as the substrate – gutter layer as it mitigates the interfacial problem noted earlier for composite membranes while still being highly permeable to minimize resistance. Hence, N2/CO2/CH4 gases were chosen as the model permeants for further composite fabrication with P84 polyimide (PI) as selective layer. Nevertheless, low surface energy of PMP limit its compatibility to form a composite layer. However, it was noted that PMP is compatible to form a bilayer through dip coating with P84 PI, without the need for pre-treatment. Hence, P84 PI of various concentration was dip coated at 5 mm/s onto PMP-based dense skin hollow fiber membrane and tested for gas permeation performance. Results showed that ideal selectivity as high as 42.36 ± 19.08 for CO2/CH4 and 18.55 ± 6.06 for CO2/N2 was achieved at 14 wt.% P84 PI coating. Nevertheless, despite of PMP’s resistibility to the harsh N-methyl-2-pyrrolidone (NMP) solvent used for P84 PI solvation, introduction of P84 PI at low concentration (2 – 10 wt.%) damages the thin, dense skin layer of the PMP’s membrane surface which jeopardize the composite’s separation performance. It is hypothesised that P84 PI’s shrinkage during drying teared the underlying PMP layer which caused this degradation. Hence, there exist a minimum P84 PI polymer concentration in which a defect free selective layer can be made (which is at about 14 wt.%). At this concentration, dip coating speed can be manipulated to obtain a thinner defect-free selective layer suitable for composite membrane fabrication, although dewetting of the coating solution still occurred and magnified as the coating thickness is reduced.
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Submitted on : Wednesday, April 27, 2022 - 9:34:04 AM
Last modification on : Thursday, April 28, 2022 - 3:35:51 AM

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Zulfida Mohamad Hafis Mohd Shafie. Polydimethylsiloxane & poly(4-methyl-1-pentene) as gutter layer and P84 polyimide coated composite hollow fiber membranes for N₂/CO₂ and CO₂/CH₄ separation. Chemical and Process Engineering. Université de Lorraine; Universiti sains Malaysia, 2021. English. ⟨NNT : 2021LORR0212⟩. ⟨tel-03652781⟩

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